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WO2024150164A1 - Dispositif de chauffage pour chauffer des gaz ou des mélanges de gaz et installation pour conduire des procédés chimiques comprenant ledit dispositif de chauffage - Google Patents

Dispositif de chauffage pour chauffer des gaz ou des mélanges de gaz et installation pour conduire des procédés chimiques comprenant ledit dispositif de chauffage Download PDF

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Publication number
WO2024150164A1
WO2024150164A1 PCT/IB2024/050285 IB2024050285W WO2024150164A1 WO 2024150164 A1 WO2024150164 A1 WO 2024150164A1 IB 2024050285 W IB2024050285 W IB 2024050285W WO 2024150164 A1 WO2024150164 A1 WO 2024150164A1
Authority
WO
WIPO (PCT)
Prior art keywords
gas
heater
reactor
electrodes
electrode
Prior art date
Application number
PCT/IB2024/050285
Other languages
English (en)
Inventor
Paolo Argenta
Enrico Malfa
Mattia BISSOLI
Ronald Victor Manuel Lopez-Gomez
Petrus Johannes JONKER
Original Assignee
Tenova S.P.A.
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Tenova S.P.A. filed Critical Tenova S.P.A.
Publication of WO2024150164A1 publication Critical patent/WO2024150164A1/fr

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Classifications

    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J6/00—Heat treatments such as Calcining; Fusing ; Pyrolysis
    • B01J6/008—Pyrolysis reactions
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J19/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
    • B01J19/087—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy
    • B01J19/088—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J7/00—Apparatus for generating gases
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
    • C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
    • C01B3/22—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of gaseous or liquid organic compounds
    • C01B3/24—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of gaseous or liquid organic compounds of hydrocarbons
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/00049—Controlling or regulating processes
    • B01J2219/00051—Controlling the temperature
    • B01J2219/00074—Controlling the temperature by indirect heating or cooling employing heat exchange fluids
    • B01J2219/00087—Controlling the temperature by indirect heating or cooling employing heat exchange fluids with heat exchange elements outside the reactor
    • B01J2219/00103—Controlling the temperature by indirect heating or cooling employing heat exchange fluids with heat exchange elements outside the reactor in a heat exchanger separate from the reactor
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
    • B01J2219/0803—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy
    • B01J2219/0805—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges
    • B01J2219/0807—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges involving electrodes
    • B01J2219/0809—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges involving electrodes employing two or more electrodes
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
    • B01J2219/0803—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy
    • B01J2219/0805—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges
    • B01J2219/0807—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges involving electrodes
    • B01J2219/0816—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges involving electrodes involving moving electrodes
    • B01J2219/082—Sliding electrodes
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
    • B01J2219/0871—Heating or cooling of the reactor
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/02—Processes for making hydrogen or synthesis gas
    • C01B2203/0266—Processes for making hydrogen or synthesis gas containing a decomposition step
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/04—Integrated processes for the production of hydrogen or synthesis gas containing a purification step for the hydrogen or the synthesis gas
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/08—Methods of heating or cooling
    • C01B2203/0805—Methods of heating the process for making hydrogen or synthesis gas
    • C01B2203/085—Methods of heating the process for making hydrogen or synthesis gas by electric heating
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/08—Methods of heating or cooling
    • C01B2203/0872—Methods of cooling
    • C01B2203/0883—Methods of cooling by indirect heat exchange
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/14—Details of the flowsheet
    • C01B2203/146—At least two purification steps in series

Definitions

  • the present invention relates to a gas or gas mixture heater for uses in process industries.
  • the present invention further relates to a plant for conducting chemical processes comprising such heater.
  • the present invention also relates to a plant and process for high efficiency production of hydrogen by pyrolysis.
  • the invention relates to producing hydrogen by pyrolysis reactions of hydrocarbons.
  • grey hydrogen wherein the production occurs by steam reforming the methane, a technology which involves a significant impact from the point of view of CO2 emissions;
  • Turquoise hydrogen providing a direct pyrolysis of methane (and/or other hydrocarbons) .
  • Electrodes made of carbon usually graphite, operating by both direct and alternate current .
  • cathode and anode are installed along axes inclined with respect to each other, such that, through their moving, moving the ends close and away, and accordingly varying the current, with the same voltage, is possible.
  • the inclination of the electrodes further accentuates the problems of mechanical resistance (by the way limiting the selection of the electrode typologies to those with higher mechanical resistance, i.e. , those made of graphite, which are notoriously more expensive than those made of prebaked carbon and those of the Soderberg type) ;
  • the indirect heating solutions require the use of a carrier gas for transferring energy.
  • a carrier gas for transferring energy.
  • such gas has a composition similar to that of the output gases, it will not be necessary to separate it from the current of products.
  • such solution reduces the yield in H2 of the process and requires having a system for separating the carrier gas from the products;
  • the main purpose of the present invention is to provide a solution for a process for high efficiency production of hydrogen, in particular turquoise hydrogen, as well as a plant for high efficiency production of hydrogen, and a reactor and a heat exchanger for high efficiency production of hydrogen, capable of solving in a unique combination the above-mentioned problems of the prior art .
  • the invention further relates to a process for high efficiency production of hydrogen as claimed in claim 16.
  • figure 1 is a schematic view of the gaseous flows in a plant according to the invention for performing a process according to the invention
  • figure 2 shows a scheme of the evolution of the temperature of the gas flow in a plant according to the invention
  • figures 3a - 3d show further evolutions of the gas flow, in particular of its composition
  • figure 4 shows a sectional view of a first non-limiting embodiment of the inventive reactor which forms part of the plant according to the invention for performing the process according to the invention
  • figures 4a - 4d are schematic views on orthogonal planes of different possible alternative embodiments of a reactor which forms part of the plant according to the invention for performing the process according to the invention
  • figure 5 shows a sectional view of a second embodiment of the inventive reactor which forms part of the plant according to the invention for performing the process according to the invention
  • figure 6 shows a sectional view of a third embodiment of the inventive
  • FG Fee Gas
  • gas or gas mixture comprising hydrocarbons, for example methane or mixtures of compounds C x H y in the state of gas or vapour;
  • the entering gas can be at least partially of non-fossil origin but produced from renewable sources, for example it can be biogas or biomethane.
  • methane comprising the alternatives set forth above.
  • the output flow is composed of acetylene C2H2, in addition to gaseous residuals, whose composition substantially depends on the components of the entering gases and on the passage through the reactor 1, and solid residuals, mainly solid-state carbon (in the following "Solid Carbon", abbreviated to SC) with different crystalline and aggregation forms, comprising the above-mentioned Carbon Black.
  • the gas to be processed in particular methane
  • the flow SI of pre-heated gas is then sent to the plasma reactor 1, where the pyrolysis reaction occurs.
  • the flow S2 at high temperature of the produced gases hydrogen, gaseous residuals typically comprising acetylene and methane, in addition to a solid part, consisting of carbon in the form of powder or the like
  • the cooled gaseous flow S3 continues to a gas/solid separator (SGS) for removing the solid part (SC) .
  • SGS gas/solid separator
  • the flow S4 depurated of the solid part is sent to a gas/gas separator (GGS) for removing the residuals of other gases deriving from the pyrolysis reaction (comprising methane and acetylene) and/or originally in the entering gas, obtaining a main flow S51 mainly composed of hydrogen and a residual flow S52, which comprises methane, acetylene and/or other (as described above) , which can be optionally recycled by making it converge in the gas flow FG to be processed.
  • the process according to the invention provides three steps (as illustrated in figure 2) a step of pre-heating the methane current, a step of reaction, and a step of cooling the produced gases, now rich in hydrogen .
  • FIG. 3a-3d An example of the evolution of the current of the gases is illustrated in the attached figures 3a-3d, showing the trend over time of the mass fraction of certain components (respectively methane CH4, hydrogen H2, acetylene C2H2, solid carbon in the form of powder or other aggregation forms) of a mass unit of gas subjected to the process according to the invention.
  • a first embodiment of the reactor according to the invention generally denoted by reference number 1
  • FIG. 1 An example of the evolution of the current of the gases is illustrated in the attached figures 3a-3d, showing the trend over time of the mass fraction of certain components (respectively methane CH4, hydrogen H2, acetylene C2H2, solid carbon in the form of powder or other aggregation forms) of a mass unit of gas subjected to the process according to the invention.
  • FIG. 4 of the attached drawings a first embodiment of the reactor according to the invention, generally denoted by reference number 1, is shown, providing an outer metal structure 100, possibly cooled by water in
  • At least one opening 120 connected to a system for feeding the gas to be treated, in this case a gas mixture containing hydrocarbons, in particular methane gas, which allows the gas to be treated to enter the reaction chamber 101, is provided.
  • a gas mixture containing hydrocarbons, in particular methane gas which allows the gas to be treated to enter the reaction chamber 101.
  • the at least one opening 120 can be made in various different manners:
  • At least one opening 130 is arranged in the lower part and is vertically facing downward (optionally the opening 130 can be arranged in the upper part, facing laterally or upward) , for the leakage of the products of the reaction, comprising a mixture of gas (comprising hydrogen and residuals of hydrocarbons and/or acetylene and possible other gases, as described above) and solid (solid carbon, SC, in the form of powder or other aggregation forms) .
  • a mixture of gas comprising hydrogen and residuals of hydrocarbons and/or acetylene and possible other gases, as described above
  • solid solid carbon, SC, in the form of powder or other aggregation forms
  • Said opening 130 is connected to the rest of the plant, not represented in figure, which comprises the systems for treating the products of the reaction (comprising cooling in a dedicated heat exchanger 4, separating the solid carbon in a gas/solid separator 2, and separating the residual methane and acetylene from hydrogen in a gas/gas separator 3 ) .
  • said structure 100 provides at least one opening 135 for introducing at least one electrode 200.
  • elements for heat insulation 140, elements for pneumatical sealing 150, adapted to prevent gas exchanges between interior and exterior of the reactor at the opening 135 for introducing the electrode 200, in particular intended to prevent air, in particular oxygen, from entering the reactor 1, and the reaction gases within the reactor 1, highly flammable gases also with explosive reactions, from leaking, are provided.
  • a fixed electrode 300 for example an anode, electrically connected with the exterior of the reactor.
  • the mobile electrode 200 in this case a cathode, is vertically arranged and there are means (not represented) for moving the same along its longitudinal axis. Furthermore, preferably, the mobile electrode 200 has a circular and full cylindrical section (i.e. , there are no longitudinal holes) .
  • the gas flow to be treated enters through the passages 120, is heated as a result of the electric arc between anode 300 and cathode 200, until activating the pyrolysis reactions.
  • the gas mixture deriving from the pyrolysis reactions is then extracted through the opening 130 which puts the reactor 1 in communication with the rest of the plant.
  • the reactor 1 of the plant according to the invention is identical to that illustrated and described with reference to figure 4, only differing in that at least one lower opening 130 is facing and addressed horizontally.
  • FIG 6 of the attached drawings a third embodiment of the reactor 1 of the plant according to the invention is shown, wherein the fixed electrode 300 (anode) is placed vertically below the mobile electrode 200. Thereby, the gases produced by the pyrolysis reactions are evacuated from the reactor 1 through the opening 160, laterally arranged below on the structure 100, connected to the rest of the plant (not shown) .
  • the anode 300 is supported by a structure 170 made of insulating material and is connected to the electric supply system through one or more connections 180.
  • a further embodiment of the reactor 1 is schematically represented in figure 7, wherein three electrodes 200 (of which one visible in the intersection plane, one represented in partial view, and a third not visible in the figures) , which are supplied by a three-phase system, wherein each electrode is connected to one of the three phases of the system.
  • the fixed conductive element 300 which forms, electrically, the star centre of the three- phase system.
  • the fixed conductive element 300 preferably made of carbon, is supported by a supporting structure 310, electrically insulated with respect to the outer metal structure 100.
  • each electrode 200 can be moved, relative to the fixed element 300, regardless of the other electrodes. This allows to carry out the adjustment of the electric arc, which strikes between each electrode 200 and the fixed conductive element 300, even in the case of electrodes vertically arranged and movable along the vertical direction.
  • the reactor 1 described above with reference to the figures of the attached drawings which forms an example of reactor to be provided in the plant according to the invention for actuating the process according to the invention, forms a system operating at high temperature ( 1200-2000 °C, preferably 1200-1500°C) with direct technology, i.e. , without a carrier gas for transporting thermal energy, wherein the energy is provided by plasma arc generated by electrodes made of carbon through which direct current (DC) or alternate current (AC) flows.
  • DC direct current
  • AC alternate current
  • the electrodes are vertically positioned and moved along their axis, and can be made of graphite, amorphous carbon or be of the Soderberg type.
  • DC Direct Current
  • the fixed element is electrically configured as a fixed "star centre", in addition to the three electrodes for the three phases, vertically mobile and independent of each other; the star centre is located in the middle between the three electrodes, therefore the electric arc strikes between each single phase (electrode) and the star centre.
  • the arcs strike between electrodes and metal bath, the latter representing the "star centre" of the circuit, while in the reactor 1 according to the invention the metal bath is replaced by the fixed conductive element.
  • a system for controlling and moving the electrodes capable of adjusting the distance between mobile and fixed electrodes (in the DC case) or between the electrodes and the star centre (in the AC case) as a function of the current and voltage parameters adapted to generate an electric arc, is provided.
  • the reactor 1 In order to ensure the operative safety related to the highly explosive/f lammable atmosphere, the reactor 1 according to the invention is provided with a sealing system for preventing air/oxygen from entering the reactor, and simultaneously the internal gases (methane, hydrogen, acetylene, etc. ) from leaking.
  • a sealing system for preventing air/oxygen from entering the reactor, and simultaneously the internal gases (methane, hydrogen, acetylene, etc. ) from leaking.
  • the above-mentioned problems 3) to 6) of the known technology are at least partially solved.
  • the vertical arrangement allows to cancel the bending stress of the electrodes due to their own weight, thus decreasing the mechanical stresses, and making it possible using electrode typologies having lower mechanical resistance and cost.
  • EAF electric arc furnaces
  • SAF submerged arc furnaces
  • a heat exchanger which forms the heat recovering system, for pre-heating the gas mixture FG (comprising, as described above, gaseous hydrocarbons C x H y , in particular methane) entering the reactor 1, using the heat of the produced gases.
  • gas mixture FG comprising, as described above, gaseous hydrocarbons C x H y , in particular methane
  • Said heat exchanger can be made according to two preferred embodiments.
  • the heat exchanger 4 is of the mobile bed type of typically spherical elements, being divided in two sections: in the first 41 (upper in figure 8) the hot gases S2 exiting the reactor 1 transfer heat to spherical elements 42, generating a flow of cooled produced gases S3 exiting the exchanger 4.
  • Said spherical elements 42 are preferably made of hard material, resistant to temperatures higher than 1200/1500/2000 °C (depending on the process temperature, the alumina can be a material usable for the elements 42) .
  • spherical elements 42 but they could be replaced by other solid elements, adapted to form a mobile bed extending in the vertical direction, even if the rounded shapes are preferred, elements which are introduced from above and which descend by gravity downward (the cooled gases are sucked at the exit of the exchanger 4 ) .
  • said spherical elements 42 In the second part 43 of the exchanger 4 (lower part in figure 8) said spherical elements 42, after being heated in the upper part 41, transfer heat to the gas flow FG entering the exchanger 4 and intended to enter the reactor 1 as a flow SI of pre-heated gas, pre-heating it.
  • the passage between the two parts 41 and 43 is made so as to allow the spherical elements 42 to pass, simultaneously preventing (or however limiting) the gases from passing between the second 43 and the first part 41.
  • a first embodiment of the exchanger 4 (mobile bed of spherical elements or of similar shape) consisting of an outer metal structure, internally coated by one or more layers, of which some consisting of refractory material and others of heatinsulating material, is illustrated; the layers can also consist of materials different from each other and can have different differentiated mechanical and thermal features (insulating or refractory) .
  • the used refractory material can be based on alumina.
  • the exchanger 4 has at least one duct 1100 for passing the spherical elements 42, substantially vertically, comprised between an inlet 1101 and an outlet 1102.
  • An upper area 1103, an intermediate or transition area 1104, and a lower area 1105 can be identified along the duct 1100.
  • the input of the spherical elements 42 occurs through at least one duct 1101', having a lower diameter than the duct 1100, extending through the upper wall of the exchanger 4, within the duct 1100, by a segment having a length Hl .
  • Said upper area 1103 comprises, in addition to the inlet 1101 of the spherical elements 42, at least one inlet 1110 for entering in the upper area the gas flow (e.g. , mixture of hydrogen, methane, acetylene, ...) coming from the reactor 1.
  • the inlet 1110 can be configurated, as commonly known, for example in a plurality of outlets in the duct 1100 evenly distributed along a cross section of the duct itself, i.e. , along the perimetral circumference of the duct at a cross section; a distribution on multiple cross sections, placed at different heights, can be also provided.
  • the upper area 1103 further comprises at least one outlet 1120 for exiting the gas flow coming from the reactor 1, arranged in the segment (having a length Hl) comprised between the bottom end part of the duct 1101' and the upper wall of the exchanger 4.
  • the gases passing in the upper area 1103 transfer heat, cooling themselves, to the spherical elements 42 which pass by gravity along the duct 1101' downwardly.
  • the lower area 1105 comprises at least one duct 1104' for entering the spherical elements coming from the transition area 1104 into the lower area 1105.
  • Said duct 1104' can have a diameter lower than the duct 1100 and extends through the upper wall of the lower area 1105 by a segment having a length H2.
  • the lower area 1105 further has at least one inlet 1130 of the gas to be treated intended for the reactor 1, which can be single, as represented in the figures, or can be configured, as known in the art, in a plurality of outlets in the duct 1130 evenly distributed along a cross section of the duct 1100. Furthermore, a distribution on multiple cross sections, placed at different heights, can be also provided.
  • the lower area 1105 provides at least one outlet 1140 of the gas to be treated directed toward the reactor 1, placed in the segment (having a length H2) comprised between the bottom end part of the duct 1102' and the upper wall of the lower area 1105 of the exchanger 4.
  • the gas to be treated receives heat, heating itself, from the spherical elements 42 previously heated in the upper area 1103, which thus are cooled in the lower area 1105.
  • the gas to be treated can reach temperatures higher than 400°C-600°C, thus allowing a partial cracking of the hydrocarbons in the heat exchanger. This allows energy consumptions of the reactor to be reduced.
  • the lower area 1105 can be conformed, in the bottom end area, in an inverted truncated cone shape, as represented in figure.
  • the transition area 1104 is identified between the connections at a lower height of the upper area 1103 (in figure, the inlet 1110 of the gases exiting the reactor 1) and the upper wall of the lower area 1105.
  • the transition area 1104 has, as represented in figure, a reduced section, with a truncated cone-shaped converging segment having an angle between axis and wall preferably lower than 20° .
  • the transition area 1104 comprises a plurality of ducts 1104' connecting the upper area 1103 to the lower area 1105, as schematically represented in figure 11.
  • a device 1303 (figure 12) for adjusting the flow of spherical elements 42, which can be made for example by a rotative valve of the known type (referred to as valve 1303 below) , is provided at the outlet 1102 of the exchanger 4.
  • the mode of managing the exchanger 4 provides that the entire flow of the spherical elements is only adjusted by the valve 1303, and that there are never free fall segments.
  • the geometry of the inner parts is shaped to keep a mass flow so as to optimize the heat transfer between gases and solids.
  • the duct 1101 ' is constantly filled with spherical elements 42, at least in the segment between the upper wall of the exchanger 4 and the bottom end part of the duct itself;
  • the upper area 1103 is constantly filled with spherical elements 42 up to the lower edge of the duct 1101';
  • the transition area 1104, comprising the duct 1104', is constantly filled;
  • the lower area 1105 is constantly filled up to the lower edge of the duct 1104' .
  • plenum A between the outer wall of the duct 1101' and the corresponding area of the inner wall of the duct 1100
  • plenum B between the outer wall of the duct 1104' and the corresponding area of the inner wall of the duct 1100.
  • this object is achieved by a system for loading the spherical elements 42 consisting in sequence from top to bottom as represented in figure 12 of :
  • a first container 1201 of the spherical elements 42 for example a silo or a hopper;
  • first sealing valve 1301 (open-close) for passing/blocking the spherical elements 42 and the gases ;
  • a second container 1202 of the spherical elements 42 for example a closed silo, connected with an internal atmosphere control system 1202' to the silo 1202, with the possibility to make vacuum conditions and/or controlled atmosphere conditions (e.g. , inert, or with nitrogen, etc. ) ; - a second sealing valve 1302 (open-close) for passing/blocking the spherical elements 42 and the gases ;
  • a third container 1203 of the spherical elements 42 for example a closed silo, directly connected to the exchanger 4 through the duct 1101' .
  • valve 1302 opening the valve 1302 for unloading the contents of the container 1202 within the container 1203, from which the spherical elements 42 flow into the exchanger through the duct 1101', with continuous flow adjusted by the valve 1303.
  • the containers 1201 and 1203 contain a variable level of spherical elements 42, and are never in conditions of absence of spherical elements 42 in the container 1203; the container 1202 alternates between a complete filling condition (when it receives the load from the container 1201) and a complete emptying condition (when pouring the load into the container 1203) .
  • the exchanger 4 there is a transition area 1104 wherein the spherical elements 42 pass from the top chamber 1103 (the spherical elements 42 receive heat from the gas current exiting the reactor 1) to a bottom chamber 1105 (the spherical elements 42 transfer heat by pre-heating the gas to be treated - typically methane - entering the reactor 1) .
  • the passage of the gas to be treated from the bottom chamber to the top chamber needs to be limited, thus maximizing its passage toward the reactor 1.
  • a suitable hydraulic/fizid- dynamic/fucidic resistance (or, in other words, pressure drop) to the passage of the gases in the transition area 1104 needs to be ensured.
  • a suitable flow of the spherical elements 42 downward needs to be ensured, avoiding obstructions in the path of the spherical elements 42 themselves. This result can be obtained by selecting an average dimension of the spherical elements 42 being suitably small both in an absolute sense and relative to the minimum dimension of the path within the exchanger.
  • the average diameter of the spherical elements 42 is lower than 50 mm/25 mm/10 mm/5 mm/1 mm, for example 6 mm, or for example 5 mm.
  • the minimum diameter of the passage needs to be at least equal to 10 times the average diameter of the spherical elements 42.
  • Another key parameter for making a suitable hydraulic resistance (or pressure drop) to the passage of the gases is the length of the transition area 1104, which needs to be preferably equal to at least 10/20/50/100/200 times the average diameter of the spherical elements 42.
  • the spherical elements 42 in addition to receiving heat from the gas current exiting the reactor 1, store on their surface at least a part of the SC in suspension in the current itself .
  • the spherical elements 42 transfer heat to the gas to be treated, pre-heating it, and passing from a temperature in the order of 1200/1500/2000 °C at the inlet of the bottom chamber to another in the order of 100 - 400°C at the end of the step of heat exchanging with the gases to be treated directed to the reactor.
  • there are spherical elements 42 which are covered by a layer of SC, and which are at a high temperature. In these conditions, if exposed to an oxidizing agent (e.g. , air) , there would be a remarkable risk of fire of the SC.
  • an oxidizing agent e.g. , air
  • means for a controlled transition, in terms of composition and temperature, toward an oxidizing atmosphere such as air are provided downstream of the valve 1303 for adjusting the flow of spherical elements 42.
  • Such means can be composed of a system conceptually similar to what is described for loading the spherical elements 42 entering the exchanger, and comprising: a first container 1204 which is always receiving the flow of spherical elements 42 from the valve 1303; a first sealing valve 1304 (open-close) for passing/blocking the spherical elements 42 and the gases ; a second container 1205, provided with an internal atmosphere control system 1205', and receiving the load of spherical elements 42 from the first container 1204; a second sealing valve 1305 (open-close) for passing/blocking the spherical elements 42 and the gases .
  • a method of evacuating the spherical elements 42 in the exchanger comprising the steps of :
  • this step preferably comprises cooling the spherical elements 42 in the container 1205, which can be performed for example by a cooled current of inert gas;
  • the container 1204 contains a variable level of spherical elements 42; the container 1205 alternates between a complete filling condition (when it receives the load from the container 1204) and a complete emptying condition (when pouring the load through the valve 1305) .
  • the spherical elements 42 can be effectively unloaded from the exchanger 4 at a safe temperature for preventing the SC from burning in air in a uncontrolled manner .
  • valve 1304 being open and the valve 1305 being closed.
  • the valve 1304 closing the valve 1304, and starting the gas managing procedure for making the material in the container 1205 inert.
  • opening the valve 1305 for unloading the container 1205. closing the valve 1305 and making the container 1205 inert.
  • the system is ready to reiterate the cycle.
  • a storage in air of the spherical elements 42 for their subsequent use in the exchanger 4 can be provided, after a suitable step of cleaning from residuals of SC.
  • means for recirculating in controlled atmosphere the spherical elements 42 from the outlet to the inlet of the exchanger 4, which can comprise cooling, cleaning from SC, and recovering it, can be provided.
  • the exchanger 4 can have a fixed bed structure (observe figures 13 and 14) , consisting of at least two units 44 and 45, which work in an alternate configuration.
  • the heat exchange means within the units 44 and 45 can be based on solids with different shapes and compositions such as for example spheres, saddles, foams, rings, honeycombs, etc. , and made of ceramic material, metal material, metal oxides (for example DRI ) .
  • the exchange means consists of ceramic spheres based on alumina resistant to high temperature (>1200 °C) having a diameter comprised between 1 and 100 mm .
  • alumina resistant to high temperature >1200 °C
  • a first step (figure 13) , the flow S2 of gases produced by the reactor 1, at high temperature, is passed through the unit 44, which undergoes heating, thus obtaining a flow S3 of cooled gases; simultaneously, the flow FG of the gas to be treated is passed through the unit 45, which has been previously heated at high temperature and which transfers heat, cooling itself, to the passing gas, which exits as a flow SI of pre-heated gas to be treated and which is sent to the reactor 1 for the pyrolysis.
  • a second step (figure 14) , the flow S2 of gases produced by the reactor 1, at high temperature, is deviated toward the unit 45, which now undergoes heating, thus obtaining a flow S3 of cooled gases; simultaneously, the flow FG of the gas to be treated is now passed through the unit 44, which has been heated at high temperature during the first step and which now transfers heat, cooling itself, to the passing gas, which exits as a flow SI of pre-heated gas to be treated and which is sent to the reactor 1 for the pyrolysis.
  • the present invention also relates to a plant for high efficiency production of hydrogen by pyrolysis of an input gas mixture comprising gaseous hydrocarbons, wherein the plant comprises:
  • thermoelectric heat exchanger 4 for pre-heating the input gas mixture and for cooling the output produced mixture; wherein furthermore the heat exchanger 4 provides one or more heat exchange and storage elements 42, 44, 45, said heat exchange and storage elements 42, 44, 45 store heat by cooling the produced mixture exiting the reactor 1 and successively or simultaneously transfer heat by preheating the gas mixture entering the reactor 1.
  • the heat exchange and storage elements 42 consist of a plurality of elements of similar shape to each other, and the exchanger 4 comprises:
  • first chamber 1103 providing at least one upper inlet 1101, placed in the top of the same, for entering the heat exchange and storage elements 42 in the exchanger 4, at least one inlet 1110 in communication with the outlet from the reactor 1 of the mixture produced in the reactor 1, such that the mixture transfers heat, cooling itself, to the heat exchange and storage elements 42, at least one outlet 1120 toward the reactor 1 of the gas mixture, at a temperature lower than that of inlet , the first chamber 1103 of the exchanger 4 being in communication with a second chamber 1105, placed at a vertical height lower than the first chamber 1103, comprising in turn at least one upper inlet for the heat exchange and storage elements 42 coming, being hot, from the first chamber 1103, at least one inlet 1130 fir the inlet of the gas mixture to be processed, such that the heat exchange and storage elements 42 transfer heat to the input gas mixture, heating it, at least one outlet 1140 of the input gas mixture in communication with the inlet of the reactor 1, at least one bottom outlet 1102 of the second chamber 1105, for exiting the heat exchange and storage
  • the heat exchange and storage elements 42 consist of at least a first and a second arrays 44, 45, permeable to the passage of the gases entering and exiting the reactor 1, wherein in a first step the gases exiting the reactor 1 pass through the first array 44, heating it, and the entering gases pass through the second array 45, heating themselves, and in a second step the two gas flows are inverted, therefore the gas flows exiting the reactor 1 pass through the second array 45, heating it, and the entering gases pass through the first array 44, heating themselves.
  • the present invention also comprises an apparatus for heating by means of an electric arc gas or gas mixtures, in particular gas mixtures to be used in plants where chemical processes are made.
  • the gas mixture to be heated can comprise hydrogen, hydrocarbons, any other gaseous compound which comprises carbon and/or hydrogen and/or oxygen and/or nitrogen, by way of non-limiting example CO, H2O, NH3 and others.
  • the apparatus object of the invention consists of a heater completely analogous to the reactor 1 previously described, uncoupled from the heat exchanger 4, such that the output gas flow is available at high temperature for uses required for example in plants for conducting chemical processes.
  • the output heated gas mixture or gas can have a composition equal or very similar to that of the input gas mixture or gas to be heated; or the output heated gas mixture or gas can have a composition different from that of the input gas mixture or gas to be heated.
  • the different composition will be related to the occurrence of possible chemical and/or physical phenomena of one or more species of input gas due to the presence of the electric arc and to high temperatures in the heater.
  • the input mixture comprises hydrocarbons
  • such hydrocarbons could be subjected to a pyrolysis process, forming compounds such as solid-state carbon, acetylene, and/or hydrogen.
  • FIG 15 of the attached drawings a first embodiment of the heater according to the invention is shown, generally indicated by reference number 1', which provides an outer metal structure 100', possibly water-cooled in a known manner, and a thermally insulating inner coating 110' .
  • the metal structure 100' of the heater 1' at least one opening 120', connected to a system for feeding the gas mixture to be heated (which can comprise hydrogen, hydrocarbons, any other gaseous compound comprising carbon and/or hydrogen and/or oxygen and/or nitrogen) , which allows the gas mixture to be heated to enter the heating chamber 101', is provided.
  • a system for feeding the gas mixture to be heated which can comprise hydrogen, hydrocarbons, any other gaseous compound comprising carbon and/or hydrogen and/or oxygen and/or nitrogen
  • the at least one opening 120' can be made in various different manners:
  • figure 15b inlets distributed along a single electrode, or on a single side with respect to a plane passing through the area of the arc and perpendicular to the axes of the electrodes
  • figure 15c inlets distributed on both sides of a plane passing through the area of the arc and perpendicular to the axes of the electrodes
  • the gas flows entering through the opening 120' have a secondary effect of cooling the electrodes, increasing their useful life and their duration. From this point of view, the solution shown in figure 4c is particularly advantageous, since it allows a cooling effect on the two sides of the electric arc.
  • At least one opening 130' is arranged in the lower part and is vertically facing downward (optionally the opening 130' can be arranged in the upper part, facing laterally or upward) , for the leakage of the heated gas mixture, which, as described above, can be a composition equal to or different from the mixture to be heated and can comprise a solid phase (solid carbon, SC, in the form of powder or other aggregation forms) .
  • Said opening 130' is connected, by suitable ducts, to the rest of the plant, not represented in figure .
  • said structure 100' provides at least one opening 135' for introducing at least one electrode 200' .
  • elements for heat insulation 140', elements for pneumatical sealing 150', adapted to prevent gas exchanges between interior and exterior of the heater at the opening 135' for introducing the electrode 200', in particular intended to prevent air, in particular oxygen, from entering the heater 1', and the gas mixture within the heater 1', which could comprise highly flammable gases also with explosive reactions, from leaking, are provided.
  • a fixed electrode 300' for example an anode, electrically connected with the exterior of the heater 1 ' .
  • the mobile electrode 200 ' in this case a cathode, is vertically arranged and there are means (not represented) for moving the same along its longitudinal axis. Furthermore, preferably, the mobile electrode 200' has a circular and full cylindrical section (i.e. , there are no longitudinal holes) .
  • the gas mixture to be heated enters through the passages 120' and is heated as a result of the electric arc between anode 300' and cathode 200' .
  • the heated gas mixture is then extracted through the opening 130' which puts the heater 1' in communication with the rest of the plant.
  • the heater 1' according to the invention is identical to that illustrated and described with reference to figure 15, only differing in that at least one lower opening 130' is facing and addressed horizontally.
  • FIG 17 of the attached drawings a third embodiment of the heater 1' according to the invention is shown, wherein the fixed electrode 300' (anode) is placed vertically below the mobile electrode 200' . Thereby, the heated gas mixture is evacuated from the heater 1' through the opening 160', laterally arranged below on the structure 100', connected to the rest of the plant (not shown) .
  • the anode 300' is supported by a structure 170' made of insulating material and is connected to the electric feed system through one or more connections 180' .
  • a further embodiment of the heater 1' is schematically represented in figure 18, wherein three electrodes 200' (of which one visible in the intersection plane, one represented in partial view, and a third not visible in figures) , which are supplied by a three-phase system, wherein each electrode is connected to one of the three phases of the system.
  • the fixed conductive element 300' which forms, electrically, the star centre of the three- phase system.
  • the fixed conductive element 300' preferably made of carbon, is supported by a supporting structure 310', electrically insulated with respect to the outer metal structure 100' .
  • each electrode 200 ' can be moved, relative to the fixed element 300', regardless of the other electrodes. This allows to carry out the adjustment of the electric arc, which strikes between each electrode 200' and the fixed conductive element 300', even in the case of electrodes vertically arranged and movable along the vertical direction.
  • the heater 1' described above with reference to figures 15, 15a, 15b, 15c, 15d, 16, 17, 18, which forms an example of heater forms a system operating at high temperature ( 1200-2000 °C, preferably 1200-1500°C) with direct technology, i.e. , without a carrier gas for transporting thermal energy, wherein the energy is provided by plasma arc generated by electrodes made of carbon travelled by direct current (DC) or alternate current (AC) .
  • DC direct current
  • AC alternate current
  • the electrodes are vertically positioned and moved along their axis, and can be made of graphite, amorphous carbon or be of the Soderberg type.
  • DC Direct Current
  • the fixed element is electrically configured as a fixed "star centre", in addition to the three electrodes for the three phases, vertically mobile and independent of each other; the star centre is located in the middle between the three electrodes, therefore the electric arc strikes between each single phase (electrode) and the star centre.
  • the arcs strike between electrodes and metal bath, the latter representing the "star centre" of the circuit, while in the heater 1' according to the invention the metal bath is replaced by the fixed conductive element.
  • a system for controlling and moving the electrodes capable of adjusting the distance between mobile and fixed electrodes (in the DC case) or between the electrodes and the star centre (in the AC case) as a function of the current and tension parameters adapted to generate an electric arc, is provided.
  • the heater 1' In order to ensure the operative safety related to the internal atmosphere, which, depending on the chemical species in the gas mixture to be heated, can be highly flammable or explosive, the heater 1' according to the invention is provided with a sealing system for preventing air/oxygen from entering the heater, and simultaneously the internal gases from leaking.
  • the vertical arrangement allows to cancel the bending stress of the electrodes due to their own weight, thus decreasing the mechanical stresses, and making it possible using electrode typologies having lower mechanical resistance and cost. Furthermore, it is also possible to have easier electrode elongating procedures, similar to those used in electric arc furnaces (EAF) and submerged arc furnaces (SAF) . Finally, making the pneumatical sealing between electrode and passage opening in the structure of the reactor is simplified.
  • the present invention also relates to a plant for conducting chemical processes comprising such a heater 1' arranged to heat a process gas or gas mixture.
  • the arrangement of the electrodes with a substantially vertical orientation and the possibility of a punctual and accurate power adjustment thereof through said system for moving the electrodes themselves allows to obtain a very advantageous reactor 1/heater 1' capable of solving the specific problems of the prior art. Furthermore, thereby, in the reactor 1/heater 1' there is a remarkable easiness and flexibility in changing the electrode, and a simplification of the sealing system for preventing oxygen infiltrations.
  • the solution according to the present invention further allows the system integration of the reactor of pyrolysis by recovering heat from the exiting hot products (gas and solids) and pre-heating entering gas.
  • This system integration allows to obtain a particularly high efficiency, due to the possibility to recover heat not only from the gases, but also, at least partially, from the solid carbon, through the particular structure of the reactor and the exchanger, and to effectively use such heat for pre-heating the entering gas.

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Abstract

La présente invention concerne un dispositif de chauffage pour chauffer un gaz d'entrée ou un mélange de gaz à chauffer par arc électrique et produire un mélange de gaz ou de gaz chauffé en sortie, ledit dispositif de chauffage (1') comprenant : une structure de confinement (100') définissant une chambre de chauffage (101'), pourvue d'ouvertures pouvant être commandées pour l'entrée (120') dudit gaz ou mélange de gaz en entrée à chauffer, pour la sortie (130') du gaz ou du mélange de gaz chauffé en sortie ; au moins une électrode (200'), passant à travers un ou plusieurs trous dans la structure de confinement (100'), et des éléments d'étanchéité (150') entre lesdits trous et ladite au moins une électrode (200') pour empêcher l'échange gazeux entre l'intérieur et l'extérieur ; au moins un élément électriquement conducteur (300') placé au moins partiellement à l'intérieur de ladite chambre de réaction (101'), ladite au moins une électrode (200') étant mobile, par rapport à d'autres électrodes (200') ou audit élément électriquement conducteur (300'), le long de son axe (X'), ledit arc électrique étant formé entre ladite ou lesdites électrodes (200') et ledit élément électriquement conducteur (300'). La présente invention concerne également une installation pour conduire des procédés chimiques comprenant un tel dispositif de chauffage d') agencé pour chauffer un gaz de traitement ou un mélange de gaz.
PCT/IB2024/050285 2023-01-12 2024-01-11 Dispositif de chauffage pour chauffer des gaz ou des mélanges de gaz et installation pour conduire des procédés chimiques comprenant ledit dispositif de chauffage WO2024150164A1 (fr)

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PCT/IB2024/050284 WO2024150163A1 (fr) 2023-01-12 2024-01-11 Installation et procédé de production à haut rendement d'hydrogène par pyrolyse

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Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
FR2181570A1 (en) * 1972-04-28 1973-12-07 Weissenburg Torsten Inter-gas heat-exchanger - with transfer medium of gravitating recycled solid granules
WO1993012030A1 (fr) * 1991-12-12 1993-06-24 Kvaerner Engineering A.S Procede de decomposition des hydrocarbures
WO2001046067A1 (fr) * 1999-12-21 2001-06-28 Bechtel Bwxt Idaho, Llc Production d'hydrogene et de carbone elementaire a partir de gaz naturel et d'autres hydrocarbures
US20070267289A1 (en) * 2006-04-06 2007-11-22 Harry Jabs Hydrogen production using plasma- based reformation
WO2014087000A1 (fr) * 2012-12-06 2014-06-12 Krones Ag Dispositif et procédé de craquage de gaz

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
FR2181570A1 (en) * 1972-04-28 1973-12-07 Weissenburg Torsten Inter-gas heat-exchanger - with transfer medium of gravitating recycled solid granules
WO1993012030A1 (fr) * 1991-12-12 1993-06-24 Kvaerner Engineering A.S Procede de decomposition des hydrocarbures
WO2001046067A1 (fr) * 1999-12-21 2001-06-28 Bechtel Bwxt Idaho, Llc Production d'hydrogene et de carbone elementaire a partir de gaz naturel et d'autres hydrocarbures
US20070267289A1 (en) * 2006-04-06 2007-11-22 Harry Jabs Hydrogen production using plasma- based reformation
WO2014087000A1 (fr) * 2012-12-06 2014-06-12 Krones Ag Dispositif et procédé de craquage de gaz

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